Electrophoretic deposition (EPD) is employed successfully in a suspension of multicomponent TiO2 nanoparticulates of different sizes and morphologies to engineer a very robust bifunctional electrode structure for dye-sensitized solar cell (DSSC) applications that shows excellent light-harvesting and photoelectrochemical performance. Aqueous-synthesized anatase nanocrystallites and sub-micrometer-sized “sea urchin”-like rutile aggregates are formulated in a stable isopropanol suspension without resorting to binders or charging agents. Interestingly, extremely robust films are obtained because of the high surface reactivity, electrophoretic mobility, and unique morphology of the rutile aggregates. DSSCs built with the newly configured bifunctional electrode yielded a record efficiency (8.59 %) for EPD-fabricated devices without resorting to mechanical compression. Such green-engineered mesoporous electrode structures can be built on both metallic and plastic substrates and can find applications in various energy and environmental fields.